期刊
CHEMICAL SCIENCE
卷 11, 期 8, 页码 2148-2154出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9sc05951b
关键词
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资金
- National Natural Science Foundation of China [21722307, 21673233, 21873016, 21688102]
- National Key R&D Program of China [2018YFA0306503]
- Chinese Academy of Sciences [XDB17010200]
- Fundamental Research Funds for the Central Universities [DUT18ZD202]
- LiaoNing Revitalization Talents Program [XLYC1907190]
Roaming is a novel mechanism in reaction dynamics. It describes an unusual pathway, which can be quite different from the conventional minimum-energy path, leading to products. While roaming has been reported or suggested in a number of unimolecular reactions, it has been rarely reported for bimolecular reactions. Here, we report a high-level computational study of roaming dynamics in the important bimolecular combustion reaction H + C2H4 -> H-2 + C2H3, using a new, high-level machine learning-based potential energy surface. In addition to the complex-mediated roaming mechanism, a non-complex forming roaming mechanism is found. It can be described as a direct inelastic collision where the departing H atom roams and then abstracts an H atom. We denoted this as collision-induced roaming. These two roaming mechanisms have different angular distributions; however, both produce highly internally excited C2H3. The roaming pathway leads to remarkably different dynamics as compared with the direct abstraction pathway. A clear signature of the roaming mechanism is highly internally excited C2H3, which could be observed experimentally.
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